Journal
ACS CATALYSIS
Volume 2, Issue 12, Pages 2537-2546Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cs300551r
Keywords
Au catalysis; AuCu alloy; ethanol oxidation; acetaldehyde; dehydrogenation; heterostructure
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Funding
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [De-AC05-00OR22725]
- U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering
- UT-Battelle, LLC
- Oak Ridge National Laboratory by the Scientific User Facilities Division, U.S. Department of Energy
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The selective oxidation of ethanol with molecular O-2 is increasingly becoming an important process to develop fine chemicals because it can be obtained from renewable biomass feedstock while reducing the demand on fossil fuels. We have synthesized silica-supported Au-Cu alloy nanoparticles, and through an oxidative dealloying process, we have developed Au-CuOx hybrid catalysts for the selective oxidation of ethanol into acetaldehyde. Using a combination of XRD, XPS, and HR-STEM experiments, we have confirmed that the active catalyst is a Au core with a thin CuOx shell. Oxidation of the AuCu/SiO2 alloy catalyst at 300 degrees C was found to produce the most active and stable catalyst for ethanol conversion (similar to 90%) with the highest selectivity (similar to 80-90%) at a reaction temperature of 200 degrees C for 50 h on-stream. TEM and XRD results show that Au-CuOx/SiO2 catalysts calcined at 300 and 500 degrees C are also more resistant to sintering during pretreatment and catalytic conditions than pure gold supported on silica. Furthermore, the silica-supported Au-CuOx catalysts (calcined at 300 and 500 degrees C) were also found to be more active and selective in the dehydrogenation of ethanol to form acetaldehyde. It is likely that the increased interfacial contact between the Au and CuOx forms the most active site on the catalyst and is responsible for the enhanced catalytic properties when compared with pure Au/SiO2.
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